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Cited by 874

The DOI matches its Crossref record; 89 of the 89 references it cites were found in a registry or an index.

Ligand Exchange and the Stoichiometry of Metal Chalcogenide Nanocrystals: Spectroscopic Observation of Facile Metal-Carboxylate Displacement and Binding

Open access
Anderson, Nicholas C., Hendricks, Mark P., Choi, Joshua J., Owen, Jonathan S.·2013·Journal of the American Chemical Society
DOI 10.1021/ja4086758
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Abstract

We demonstrate that metal carboxylate complexes (L-M(O2CR)2, R = oleyl, tetradecyl, M = Cd, Pb) are readily displaced from carboxylate-terminated ME nanocrystals (ME = CdSe, CdS, PbSe, PbS) by various Lewis bases (L = tri-n-butylamine, tetrahydrofuran, tetradecanol, N,N-dimethyl-n-butylamine, tri-n-butylphosphine, N,N,N',N'-tetramethylbutylene-1,4-diamine, pyridine, N,N,N',N'-tetramethylethylene-1,2-diamine, n-octylamine). The relative displacement potency is measured by (1)H NMR spectroscopy and depends most strongly on geometric factors such as sterics and chelation, although also on the hard/soft match with the cadmium ion. The results suggest that ligands displace L-M(O2CR)2 by cooperatively complexing the displaced metal ion as well as the nanocrystal. Removal of up to 90% of surface-bound Cd(O2CR)2 from CdSe and CdS nanocrystals decreases the Cd/Se ratio from 1.1 ± 0.06 to 1.0 ± 0.05, broadens the 1S(e)-2S(3/2h) absorption, and decreases the photoluminescence quantum yield (PLQY) from 10% to <1% (CdSe) and from 20% to <1% (CdS). These changes are partially reversed upon rebinding of M(O2CR)2 at room temperature (∼60%) and fully reversed at elevated temperature. A model is proposed in which electron-accepting M(O2CR)2 complexes (Z-type ligands) reversibly bind to nanocrystals, leading to a range of stoichiometries for a given core size. The results demonstrate that nanocrystals lack a single chemical formula, but are instead dynamic structures with concentration-dependent compositions. The importance of these findings to the synthesis and purification of nanocrystals as well as ligand exchange reactions is discussed.

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Metadata

Authors
Anderson, N. C., Hendricks, M. P., Choi, J. J., & Owen, J. S.
Venue
Journal of the American Chemical Society
Publisher
American Chemical Society (ACS)
Published
2013-11-26
Volume
135
Issue
49
Pages
18536-18548
ISSN
  • 0002-7863 (ISSN-L)
  • 1520-5126
DOI
10.1021/ja4086758
OpenAlex
W1992238598
Cited by
874
References
89
FWCI
26.35
Type
journal article
Language
en
Open access
green

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